The present invention discloses a preparation method of anode active material of a rechargeable aluminum secondary battery, the secondary battery using the anode active material and a preparation method of the secondary battery. The invention aims to provide a high energy aluminum secondary battery of which anode active material has simple preparation process, low cost, no pollution and good circularity and a preparation method of the high energy battery. The anode active material is prepared by adopting a high temperature high pressure inlay and penetrating process to ensure sulfur in carbon-sulfur mixture with sulfur (S8) or sulfenyl compounds to inlay and penetrate into the surface of carbon-base and micropores at 90-300 DEG C and 320-800 DEG C under the pressure of 0.01-5 MPa. The aluminum secondary battery contains an anode prepared by the anode active material, a aluminum cathode and a aluminum electrolyte system. The products of the present invention can be used as power batteries and energy-storage batteries to be widely used in electric bicycles, electric cars, emergency power supplies, peak value adjusting systems of power station and energy-storage systems of new energies such as solar energy, wind energy and the like, and has very broad development prospect.